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The Journal of Chemical Physics

Condensation limited cooling in supersonic expansions

Matthias Hillenkamp, Sharon Keinan, Uzi Even

Published May 8, 2003• 133 citations
Publisher

Abstract

Supersonic expansions of pure and seeded rare gases have been investigated experimentally, measuring the translational and rotational temperatures. The lowest achievable translational temperature in the jet depends on both gas properties as well as on experimental boundary conditions like nozzle shape and nozzle–skimmer distance. We show that there is a limit to the lowest temperature achieved, under practical conditions, set by condensation in the jet. A large cluster binding energy enhances the formation of clusters and they release their condensation energy into the beam. The spatial confinement of the jet extends to long distances, and is sensitive to the shape of the nozzle. The confined jet forms a narrow cone of high intensity, and results in increased collision probability and cluster formation.

DOI
10.1063/1.1568331

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Supersonic expansions of pure and seeded rare gases have been investigated experimentally, measuring the translational and rotational temperatures. The lowest achievable translational temperature in the jet depends on both gas properties as well as on experimental boundary conditions like nozzle shape and nozzle–skimmer distance. We show that there is a limit to the lowest temperature achieved, under practical conditions, set by condensation in the jet. A large cluster binding energy enhances the formation of clusters and they release their condensation energy into the beam. The spatial confinement of the jet extends to long distances, and is sensitive to the shape of the nozzle. The confined jet forms a narrow cone of high intensity, and results in increased collision probability and cluster formation.
The mathematical term for the mean flow velocity in supersonic beams of ideal gases is extended to include real gas properties. This procedure yields an explicit dependence of the flow velocity on pressure, as observed in recent experiments of free jet expansions. Applied to stagnation conditions slightly above the critical point, the model suggests that seeded high-pressure jet expansions might be suitable for slowing down virtually any molecule with maximum efficiency. Moreover, we discuss the consequence of a pressure-dependent flow velocity v0{v}_{0}v0​ for the speed ratio $S={v}_{0}/\ensuremath{\Delta}{v}_{\ensuremath{\parallel}}$ with respect to collisional cooling and suggest to use the velocity spread $\ensuremath{\Delta}{v}_{\ensuremath{\parallel}}$ as a more nonambiguous measure of translational temperature in high-pressure jet expansions.
Low energy (thermal) free jet (supersonic) molecular beams are used in a range of applications from surface science and surface deposition to quantum coherence and gas kinetics experiments. A free jet molecular beam is created by a gas expansion from a high pressure reservoir through a small aperture (nozzle). The nozzle typically has a diameter of 2-20 μm. The central part of the beam is selected using a skimmer, typically up to 500 μm in diameter. Recent years have seen the introduction of highly spatially confined beam sources based on micrometer skimmers and micrometer or even sub-micrometer nozzles. Such sources have been applied, for example, in the investigation of superfluidity and in neutral helium microscopy. However, up till now no source design allowing the precise positioning of the micro-skimmer relative to the nozzle has been available. This is an important issue because the relative position of skimmer and nozzle can influence the beam properties considerably. Here we present the design and implementation of a new molecular beam source, which allows an automatized, 50 nm precision positioning of the skimmer relative to the nozzle. The source is liquid nitrogen cooled and the temperature can be controlled between 110 K and 350 K with a temperature fluctuation of less than ±0.1 K over several hours. Beam intensity measurements using a 5 μm nozzle and a skimmer 5 μm in diameter are presented for stagnation pressures po in the range 3-180 bars. A 2D beam profile scan, using a 9.5 μm skimmer and a 5 μm nozzle is presented as a further documentation of the versatility of the new design and as an illustration of the influence of the relative skimmer-nozzle position on the beam properties.
We have found recently that, in a supersonic expansion of a mixture of two monoatomic gases, the parallel temperatures of the two gases can be very different. This effect is large if the seeded gas is highly diluted and if its atomic mass is considerably smaller than the one of the carrier gas. In the present paper, we present a complete derivation of our theoretical analysis of this effect. Our calculation is a natural extension of the existing theory of supersonic cooling to the case of a gas mixture, in the high dilution limit. Finally, we describe a set of temperature measurements made on a beam of lithium seeded in argon. Our experimental results are in very good agreement with the results of our calculation.
Stable van der Waals clusters of tryptophan molecules, (Trp) n , of up to n=5, were produced in a seeded supersonic beam expansion from a laser desorption nozzle source. Translational beam temperatures of van der Waals tryptophan clusters were measured using a fast optical imaging device. Estimated beam temperatures in carrier argon gas were 27 K for tryptophan dimers (n=2) and 41 K for tryptophan trimers (n=3). A preliminary experiment showed that no significant difference was observed in the yield of van der Waals clusters for L-, D- and racemic-tryptophan molecules.
An ultra-cold molecular plasma with extraordinarily long lifetime (~0.5 ms) is generated under strong collisional cooling conditions in the expansion region of a seeded supersonic jet expansion close to the nozzle. A resonant two-photon one-color laser process excites para-difluorobenzene molecules into the high-n Rydberg threshold region. Disorder heating during plasma formation is quenched by the high collision rate in the expansion, which keeps the ions at the translational jet temperature of 0.2K-0.7K. The Coulomb coupling parameter \Gammai for the ions is expected to be ca. 230-820.
Clusters of He atoms formed in a supersonic free jet expansion have been studied by electron-bombardment ionization and mass spectrometry. Distinct magic-number enhancements of ion intensity are observed for clusters of 7, 10, 14, and 30 atoms for both helium isotopes, and for 23 atoms of 4He^{4}\mathrm{He}4He. Dramatic differences in the onset of cluster formation between the two isotopes may be related to the stability of 4He^{4}\mathrm{He}4He dimers.